Prediction Challenge: Simulating Rydberg Photoexcited Cyclobutanone with Surface Hopping Dynamics based on Different Electronic Structure Methods

This datasets contains the initial conditions and trajectories for the decoherence-corrected fewest-switch surface hopping (DC-FSSH) dynamics simulations of photo-excited cyclobutanone to the S2 Rydberg state using different electronic structure methods. We performed dynamics simulations using nonadiabatic coupling vectors (NACV) as obtained by solving the time-independent Schrödinger equation and also with approximated time-dependent Baeck-An (TDBA) couplings.  

The repository contains the following five directories: 

Structures_MCSCF: MCSCF optimized Cartesian coordinates of the electronic states minima and the minimum energy conical intersections between the states; 

Set1_MCSCF_NACV: Initial Conditions and Trajectories of DC-FSSH with NACV and multiconfigurational self-consistent field (MCSCF);

Set2_MCSCF_TDBA: Trajectories of DC-FSSH with TDBA and MCSCF;

Set3_TDDFT_TDBA: Initial Conditions and Trajectories of DC-FSSH with TDBA and time-dependent density functional theory (TDDFT) for excited states and DFT for the ground state;

Set4_MRCI-ODM3_TDBA: Initial Conditions and Trajectories of DC-FSSH with NACV and multireference configuration interaction (MRCI) based on the semiempirical orthogonalization and dispersion corrections method ODM3;

Set5_ADC2_TDBA: Initial Conditions and Trajectories of DC-FSSH with TDBA and algebraic diagrammatic construction to the second-order [ADC(2)] [ADC2-TDBA].

Each Set has its own initial conditions for dynamics (geometry and velocities) sampled from a marginal Wigner distribution of the quantum harmonic oscillator in the electronic ground state equilibrium geometry using the nuclear ensemble approach. 

The initial conditions and dynamics simulations were done using the Newton-X CS suite of programs (version 2.7). MCSCF calculations were carried out using Columbus software (version 7.2.2, Sept. 2022). The DFT and TDDFT calculations were done using ORCA v5.0.4. MRCI-ODM3 semiempirical calculations are performed with MNDO program. ADC(2) calculations are done by using Turbomole v7.6 program.